As a true freshman at North Carolina in 2018, Williams played in 11 games, rushing 43 times for 224 yards and five touchdowns. As a sophomore in 2019, he played in all 13 games and shared carries with Michael Carter. He ran for 933 yards on 166 carries with five touchdowns. Williams returned to North Carolina in 2020 and again shared carries with Carter. Throughout the 2020 season, Williams was statistically one of the top running backs in the country. Williams' name was mentioned during the season as a "dark horse" candidate for the 2020 Heisman Trophy. Against Miami (FL), Williams and backfield counterpart Carter combined for an NCAA-record 544 rushing yards as a duo in the Tar Heels' 62–26 blowout victory. Williams and Carter were both named to the 2020 Pro Football Focus First-team All-America at the running back position. PFF also named him the 2020 ACC Football Player of the Year with a record-breaking 95.9 PFF rushing grade, the highest rushing grade in a single season since the site began covering college players.
Overall, Williams finished his rookie season appearing in all 17 games (one start) and recorded 203 carries for 903 yards (4.4 YPC) and four rushing touchdowns plus 43 receptions for 319 yards and three receiving touchdowns. He was named to the PFWA All-Rookie Team.
In Week 1, Williams had 108 scrimmage yards and a lost fumble in the 16–17 loss to the Seattle Seahawks. In the loss, he had 11 receptions. During Week 4 against the Las Vegas Raiders, Williams went down with a knee injury and left the game. It was later revealed that he suffered tears to the ACL, LCL, and posterolateral corner. The injury prematurely ended his 2022 season.
In the 2023 season, Williams had 217 carries for a team-high 774 rushing yards and three rushing touchdowns to go with 47 receptions for 228 receiving yards and two receiving touchdowns in 16 games and 13 starts.
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